He will join the Tricolours on a three-year deal from 2024.
The 47-year-old was sacked by the Titans in June, but has since been a coach in demand.
Holbrook had a hugely successful stint with St Helens in Super League where he won the title in 2019. In the last few weeks he was on the verge of joining the Warrington Wolves as head coach and had an offer to join Canterbury as an assistant to Cameron Ciraldo.
The lure of the Roosters, where he was Robinson's assistant from 2014 to 2017, won him over.
"I was there seven years ago and I learned a lot there before I went to St Helens and then to the Gold Coast," Holbrook told AAP.
"Having worked with Trent before is a big plus and knowing where they need to improve, and where I can add some value, was appealing to me.
"Trent is a very intelligent coach and I also see myself learning a lot more when I am there.
"The Roosters are such a well run organisation and I am looking forward to getting back there."
Holbrook said it was difficult to turn down Warrington and the Bulldogs.
"I was very close to going back to England because I have a lot of fond memories and loved it over there. I was close to going and it was really difficult not to," he said.
"With the Bulldogs I was fortunate enough to have a chat to Cameron and Phil Gould and I really like what they are doing there and what they are building towards.
"It excited me to possibly go there but in the end the fact that I have been at the Roosters and know how they operate meant it was the right decision to make."
Holbrook's former position at Gold Coast will be taken by incoming coach Des Hasler from 2024. Jim Lenihan, Holbrook's former assistant, is the interim for the rest of this season.
"It is tough when anyone is in the position I was (at the Titans) when you are planning long-term for the future, doing your best to sign blokes and thinking you are going to be part of that," said Holbrook, who was blindsided by his removal but just glad his future is now sorted.
"When you are not and someone else gets the rewards that is hard to take, but you just have to move on. I haven't enjoyed the speculation around where I am going but I can't control that.
"At least now it is all sorted and I can just get on with it."
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