After three successive half centuries in the back-to-back Twenty20 matches in Florida and the first ODI on Thursday Gayle again showed the local fans what they had been missing after 12 months of international exile.
His contribution of 125 runs, featuring nine sixes, from 107 balls and with Samuels compiling 101 off 103 balls, lifted West Indies to 315 for five.
New Zealand were always going to be struggling to match that total and despite half centuries from BJ Watling, Martin Guptill and Kane Williamson were bowled out for 260 off 47 overs.
Saturday's result gave the hosts a 2-0 lead in the five match series which they can seal in St Kitts on Wednesday.
For Gayle this was his 20th ODI ton, a new West Indian record, surpassing the previous record set by Brian Lara.
He was prevented beating his career-best score of 153 when in the 38th over one of his shots landed in the hands of deep midwicket.
For man of the match Samuels this was his third ODI century.
The Kiwis's Rob Nicol fell early after hitting a couple of boundaries, Daniel Flynn produced 62, and whyile both Kane Williamson and BJ Watling compiled half centuries the visitors were beaten comfortably.