Born into a musical family, Charu Hariharan is the daughter of Dr. B. Arundhati, reputed playback and classical musician and T. S. Hariharan. Being exposed to music from a young age, she initially learned from her grandfather, Sri Bhagavatheeswara Iyer and later from her mother. Not just restricting herself to singing alone, she had an equal flair for percussions as well. Hence, she began learning mridangam from her guru, Sri Mannarkoil J. Balaji since she was 10 years old.

She has been awarded the CCRT (Central Govt) Scholarship for mridangam and was highly appreciated for being one of the very few percussionists.