Khan held an hour-long 'satsang' session before over 150 inmates in the women's section of the jail, the country's biggest prison.
She started her spiritual session with "Ae Malik Tere Bande Hum", aimed to bring out the negative flow of thoughts from the prisoners, and had the prisoners singing along with enthusiasm.
Khan has turned into a spiritual guru and holds satsangs and delivers spiritual discourses in different jails of the country.
"I draw inspiration from spiritual guru Satya Sai Baba and am here to promote harmony, humanity and spirituality," Khan told after the event.
Khan, who made her debut in 1989 with the foot tapping number "Khula Thala Chod Aayi" and is known for the hit "Jimmy Jimmy Jimmy Aaja" number of the film "Disco Dancer", is now into singing devotional songs for prisoners.
"I am on a national peace tour and have done five such satsangs in different jails of Maharashtra to spread the lessons of spirituality and humanity," said Khan.
The pop diva has also met many of the victims of the July Mumbai train bombings that killed nearly 200 people and injured hundreds.
Khan said her aim was to help inmates gain inner peace by forgetting the tough circumstances of everyday life.
The women inmates of Tihar actively took part as Khan sang "Jyot se Jyot Milate Chalo, Prem Ki Ganga Bahate Chalo" and "Jhulae LaL".
"Such sessions of satsang should happen more frequently as it helps us connect with god," said Jasbir Kaur, a prisoner charges with cheating and fraud.
"We feel a sense of happiness after the satsang and hope that more such sessions will be organised in the jail," she added.
"It has been a great experience for us and we are drawn towards religion," said Indira Bramhabhat, who is serving a sentence on charges of dowry harassment.
However, there was one prisoner who was not as happy.
Darshna said: "If we are not happy from within, there is no use of such events because they do not help heal the wounds." She said she was missing her family and wanted to meet them.
Before leaving the jail, Khan wished the inmates good luck for their early release.
B.K Gupta, director general Tihar Jail, was very impressed with Khan's singing. "The satsang was impressive and would help inmates to be more positive towards life," he said. He promised more such events in the future.