Zozulya, 27, spent just 24 hours on loan at the Madrid club last month before being recalled by Betis.
Zozulya, 27, spent just 24 hours on loan at the Madrid club last month before being recalled by Betis after Rayo fans greeted his arrival with banners reading: "Vallekas is not the place for Nazis."
"Real Betis, Roman Zozulya and Rayo Vallecano have reached an agreement to end the contract between the three parties on the transfer of the player to Rayo Vallecano," said the second-division Madrid club in a statement.
"Zozulya will train with Real Betis in the expectation of studying the different possibilities for the player to join another team."
Zozulya has insisted he was "not linked to or a supporter of any paramilitary or neo-Nazi group."
However, he did admit to "collaborating with the Ukrainian army to help protect his country."