"Myself and Jermain worked well together. I was really pleased with how it went," said ex-Liverpool striker Crouch.
"Three goals in one game together isn't a bad start. Hopefully we can continue like that."
The striker was sold by Redknapp to Aston Villa for £5million to finance Portsmouth's 2003 promotion campaign and then bought by Liverpool for £7million when the manager was at St Mary's and trying to save Saints from relegation.
"Come the start of the season I'm sure we will know each others' game inside out. That will prove to be good for Portsmouth.
"It's the first time we've played together for a club and we enjoyed it."
Defoe, Pompey's record buy last season at £7.5million from Spurs, said: "Me and Crouchie linked up well.
"I've played with him only a few times before at England senior and Under-21 level but we work well together.
"For a big man he has great feet. He is someone I can definitely hook up with. He has played at the top level, he is a good footballer and he is very clever.
"Now we are really looking forward to the season. I'm happy with the way I got my goal. It shows we can play together."