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There is a NPC in Hoenn who does serve the slight purpose of healing your Pokemon when you are north of the desert, but she is pretty memorable to me because many a times I have been caught in an endless cycle of her healing my Pokemon. She always says something like 'You still look tired, rest some more!' and this keeps me from just mashing the A button while talking to her.
Something would be memorable to me if they didn't all say something stupid and pointless!
The memorable NPC to me, although, you do battle her is in the water right after Dewford town.
"My boyfriend lied, he says I look good in a Bikini."
WHAT GAMEFREAK?! YOU'RE PUTTING INSECURITIES IN POKEMON.
The guy on Mauville's Bicycle Road in Hoenn who just says "Rydel Rydel Rydel Rydel Rydel Rydel Rydel Rydel Rydel Rydel" over and and over. Why did Gamefreak think this guy was necessary? You have no idea how many times I've accidentally talked to him and even gone into a continous loop of him saying "Rydel" over and over. He's both the most annoying NPC and the most pointless.
He might be a trainer, but Fisherman Ralph on Route 32 in the Johto is always memorable. Instead of calling you about his pokemon, he calls to ask how you and your mom are doing. He reminds you that your mom is home alone, and would love to hear you call her.