Here are some Sentai villains I believe deserve to be mentioned for their infamous evil laughs in no particular order:
Ahames, the Queen of Amazo. Most of Gozma are not even close to her cruelty and sadism.
Radiguet- He had the most disturbing evil laugh which specified that he really did something very NASTY for the whole episode. In fact, it's his happiness to really cause sufferings to people and PROLONG it. It was so boisterous and scary. Maybe he should be given the most evil laugh award.
Shaddam- While Gorma XV was scary, Shaddam is the really big evil of Dairanger. Plus it does help to know he's very uncaring even to his twin sons Kou and Akomaru.
Grandienne- One has to realize that she like Shaddam doesn't care about her own children.
Long- He laughs like any typical sadist. Though not as loud as Radiguet, one can tell he's already killed enough to satisfy him.
Akumaro- I don't know if he should be here. Some of my followers think he's a lame villain but his "ohohohoho" is just creepy IMO.
Ahames, the Queen of Amazo. Most of Gozma are not even close to her cruelty and sadism.
Radiguet- He had the most disturbing evil laugh which specified that he really did something very NASTY for the whole episode. In fact, it's his happiness to really cause sufferings to people and PROLONG it. It was so boisterous and scary. Maybe he should be given the most evil laugh award.
Shaddam- While Gorma XV was scary, Shaddam is the really big evil of Dairanger. Plus it does help to know he's very uncaring even to his twin sons Kou and Akomaru.
Grandienne- One has to realize that she like Shaddam doesn't care about her own children. 
Long- He laughs like any typical sadist. Though not as loud as Radiguet, one can tell he's already killed enough to satisfy him.