Raman married Lokasundari Ammal, daughter of S. Krishnaswami Iyer who was the Superintendent of Sea Customs at Madras, in 1907. The wedding day is popularly recorded as on 6 May, but Ramans great-niece and biographer, Uma Parameswaran, revealed a factual date of 2 June 1907. It was a self-arranged marriage and his wife was 13 years old. (Sources are contradicting on her age as her birth year is specified as 1892, which would make her about 15 years of age; but Parameswaran affirmed the 13-year, corroborated by her obituary in Current Science that mentioned her age as 86 on her death on 22 May 1980.) His wife later jokingly recounted that their marriage was not so much about her musical prowess (she was playing veena when they first met) as "the extra allowance which the Finance Department gave to its married officers." The extra allowance refers to an additional INR 150 for married officers at the time. Soon after they moved to Calcutta in 1907, the couple were accused of converting to Christianity. It was because they frequently visited St. Johns Church, Kolkata as Lokasundari was fascinated with the church music and Raman with the acoustics.
They had two sons, Chandrasekhar Raman and Venkatraman Radhakrishnan, a radio astronomer. Raman was the paternal uncle of Subrahmanyan Chandrasekhar, recipient of the 1983 Nobel Prize in Physics.
Throughout his life, Raman developed an extensive personal collection of stones, minerals, and materials with interesting light-scattering properties, which he obtained from his world travels and as gifts. He often carried a small, handheld spectroscope to study specimens. These, along with his spectrograph, are on display at IISc.
Lord Rutherford was instrumental in some of Raman's most pivotal moments in life. He nominated Raman for the Nobel Prize in Physics in 1930, presented him the Hughes Medal as President of the Royal Society in 1930, and recommended him for the position of Director at IISc in 1932.
Raman had a sense of obsession with the Nobel Prize. In a speech at the University of Calcutta, he said, "I'm not flattered by the honour [Fellowship to the Royal Society in 1924] done to me. This is a small achievement. If there is anything that I aspire for, it is the Nobel Prize. You will find that I get that in five years." He knew that if he were to receive the Nobel Prize, he could not wait for the announcement of the Nobel Committee normally made towards the end of the year considering the time required to reach Sweden by sea route. With confidence, he booked two tickets, one for his wife, for a steamship to Stockholm in July 1930. Soon after he received the Nobel Prize, he was asked in an interview the possible consequences if he had discovered the Raman effect earlier, which he replied, "Then I should have shared the Nobel Prize with Compton and I should not have liked that; I would rather receive the whole of it."