Talajic, voted Asia's best coach in 2010-11 by Al Jazeera Sports, lasted just four matches at Kalba as his team lost all their three matches in the Pro League without scoring a goal.
Benzarti spent last season at Emirates, but could not help them avoid relegation. He remained at the team's helm for last month's promotion playoffs, but the Ras Al Khaimah club failed in their bid to return to the Pro League despite assembling a strong squad.
"I am happy to be back in the Pro League and I will do my best to rescue Kalba from their current position," Benzarti said. "We have good players in the team and we just need to find our game on the pitch."
Follow us @SprtNationalUAE