In 1902, Raman joined Presidency College in Madras where his father was a lecturer in mathematics and physics. In 1904 he passed his Bachelor of Arts examination of University of Madras. He stood first and won the gold medal in physics. In 1907 he gained his Master of Sciences degree with the highest distinctions from University of Madras.
He was married on 6 May 1907 to Lokasundari Ammal (1892–1980). They had two sons, Chandrasekhar and radio-astronomer Radhakrishnan.
Raman had association with the Banaras Hindu University in Varanasi; he attended the foundation ceremony of BHU and delivered lectures on "Mathematics" and "Some new paths in physics" during the lecture series organised at BHU from 5 to 8 February 1916. He also held the position of permanent visiting professor at BHU.
In the year 1917, Raman resigned from his government Service after he was appointed the first Palit Professor of Physics at the University of Calcutta. At the same time, he continued doing research at the Indian Association for the Cultivation of Science (IACS), Calcutta, where he became the Honorary Secretary. Raman used to refer to this period as the golden era of his career. Many students gathered around him at the IACS and the University of Calcutta. In 1926 Prof. Raman established the Indian Journal of Physics and he was the first Editor. The second volume of the Journal published his famous article "A New Radiation", reporting the discovery of Raman Effect.
During a voyage to Europe in 1921, Raman noticed the blue colour of glaciers and the Mediterranean sea. He was motivated to discover the reason for the blue colour. Raman carried out experiments regarding the scattering of light by water and transparent blocks of ice which explained the phenomenon.
India celebrates National Science Day on 28 February of every year to commemorate the discovery of the Raman effect in 1928.
Raman spectroscopy came to be based on this phenomenon, and Ernest Rutherford referred to it in his presidential address to the Royal Society in 1929. Raman was President of the 16th session of the Indian Science Congress in 1929. He was conferred a knighthood, and medals and honorary doctorates by various universities. Raman was confident of winning the Nobel Prize in Physics as well but was disappointed when the Nobel Prize went to Owen Richardson in 1928 and to Louis de Broglie in 1929. He was so confident of winning the prize in 1930 that he booked tickets in July, even though the awards were to be announced in November, and would scan each day's newspaper for announcement of the prize, tossing it away if it did not carry the news. He did eventually win the 1930 Nobel Prize in Physics "for his work on the scattering of light and for the discovery of the Raman effect". He was the first Asian and first non-white to receive any Nobel Prize in the sciences. Before him Rabindranath Tagore (also Indian) had received the Nobel Prize for Literature in 1913.
"At the end of the 1930s and the beginning of the 1940s, Scientists observed diffuse spots in X-ray Laue photographs that were difficult to explain theoretically. Already at this stage, Chandrasekhara Venkata Raman suggested a theory of his own and criticised alternative solutions that were largely based on thermal theories proposed by Max Born and Peter Debye. This led to a conflict between Born and Raman. In this dispute, Born received support from the British crystallographer Kathleen Lonsdale. The dispute between Raman and Born involved scientific as well as social elements. Whereas Raman's support came mainly from his own experiments and from his colleagues in Bangalore, Born used his social and professional network to enlist Scientists as allies for his cause. Although initially, in the early 1940s, Born's theory was not generally accepted even in England, he eventually succeeded in marginalising the rival theory of Raman. The controversy has often been dealt with by physicists and historians of science, who, however, have too often relied on Born's autobiographical work. As has been shown, parts of this work, especially as it relates to Born's Indian visit and his contact with Raman, need careful and critical reading. In particular, the issue of Raman's resignation from the directorship of the IIS had nothing to do with Born's stay in India, such as indicated in his autobiography.". Up to some extent, this controversy led to the fact that Max Born had to wait for the Nobel Prize.
Raman was succeeded by Debendra Mohan Bose as the Palit Professor in 1932. In 1933, Raman left IACS to join Indian Institute of Science in Bangalore as its first Indian Director. Other investigations carried out by Raman were experimental and theoretical studies on the diffraction of light by acoustic waves of ultrasonic and hypersonic frequencies (published 1934–1942), and those on the effects produced by X-rays on infrared vibrations in crystals exposed to ordinary light.
He also started the company called Travancore Chemical and Manufacturing Co. Ltd. (now known as TCM Limited) which manufactured potassium chlorate for the match industry in 1943 along with Dr. Krishnamurthy. The Company subsequently established four factories in Southern India. In 1947, he was appointed as the first National Professor by the new government of Independent India.
Two days before Raman died, he told one of his former students, "Do not allow the journals of the Academy to die, for they are the sensitive indicators of the quality of science being done in the country and whether science is taking root in it or not." That same evening, Raman met with the Board of Management of his Institute and discussed (from his bed) with them any proceedings with regards to the Institute's management. Raman died from natural causes early next morning on 21 November 1970.
Raman was the paternal uncle of Subrahmanyan Chandrasekhar, who later won the Nobel Prize in Physics (1983) for his discovery of the Chandrasekhar limit in 1931 and for his subsequent work on the nuclear reactions necessary for stellar evolution.
In the past, several questions were raised about Raman not sharing the Prize with the Russian Scientists G.S. Landsberg and L.I. Mandelstam, who had observed the same effect in the case of crystals. According to the Physics Nobel Committee: (1) The Russians did not come to an independent interpretation of their discovery as they cited Raman's article. (2) They observed the effect only in crystals, whereas Raman and K.S. Krishnan in solids, liquids and gases. With that, he proved the universal nature of the effect. (3) The uncertainties concerning the explanation of the intensity of Raman- and Infrared lines in the spectra could be explained during the last year. (4) The Raman method has been applied with great success in different fields of molecular physics. (5) The Raman effect has effectively helped to check the actual problems of the symmetry – properties of molecules thus the problems concerning the nuclear-spin in the atomic physics." The Nobel Committee proposed Raman's name to the Swedish National Academy of Sciences, Stockholm, for the Nobel Prize for the year 1930.