Alpert worked closely with Dr. Timothy Leary at Harvard, where the two conducted many experiments on the effects of LSD. The pair were dismissed from the university in 1963 due to their controversial research. They relocated, and continued their experiments at a private mansion in New York (see LSD).
In 1967, Alpert travelled to India, where he became heavily involved in meditative practice and yoga. After meeting and becoming a devotee of Neem Karoli Baba, a Hindu guru in Uttar Pradesh, he changed his name to Ram Dass, meaning servant of God.
Upon his return to the United States, Alpert founded several organizations dedicated to expanding spiritual awareness and promoting spiritual growth.