Eyewitness Brydon Tarafa, told The Daily Mail he was in his nearby apartment when he heard a man shout, "Jesus Christ is born", followed by a woman screaming.
Another eyewitness, George Huckado, saw the attack from his window and heard the man shout, "Get out, devils! I cast you out, devils! In the name of Jesus Christ, I cast you out!"
"The girl was making a lot of noise, screaming," he said.
"I saw something sparkly going up and down. ... I called 911, I was begging them to come," he told The New York Post.
Police have not released the name of the man, who has been taken to Columbia Presbyterian Hospital for psychiatric evaluation.
Freeman, who took Hines as his date to the 2005 Golden Globe Awards, has paid tribute to the 33 year old, who was the granddaughter of the actor's first wife, Jeanette Adair Bradshaw.
In a statement to Gossip Cop, The Shawshank Redemption star wrote: "The world will never know her artistry in talent, and how much she had to offer.
Her friends and family were fortunate enough to have known what she meant as a person. Her star will continue to shine bright in our hearts, thoughts and prayers. May she rest in peace."
Hines' death emerges three years after Freeman famously slammed reports suggesting they were romantically involved amid false claims they were preparing to wed, blasting the allegations as "defamatory fabrications".
The 78-year-old was married to Adair Bradshaw from 1967 to 1979. His second marriage, to Myrna Colley-Lee, ended in 2010 after 26 years.
- WENN