2006年，为配合NDS版（钻石、珍珠版）的上市，TV动画同步推出全新系列《神奇宝贝钻石&珍珠》（Pokémon Diamond & Pearl，简称DP）。对战开拓区篇结束后，小遥为了独自挑战城都地区的华丽大赛和小智告别，小胜回到了橙华道馆，小刚也回家去了。小智则受到了小茂的激励，独自带着皮卡丘和偷渡的长尾怪手前往神奥地区挑战联盟。
新登场的女主角小光，其蓝本取自电玩NDS版。为了成为顶尖协调训练家，小光从家乡双叶镇来到了位于真砂镇的山梨研究所领取最初的神奇宝贝。而同一时间，小智也抵达神奥地区，并在那里和小刚再度会合。机缘巧合，小光救了被火箭队抓走的皮卡丘，三人就一同结伴旅行，展开了新的旅程。
《神奇宝贝珍珠&钻石》每周四在日本首播。台湾也由中视进行转播，网络上能够找到前105集的国语配音。

Renton, son of scientists, and Eureka, a girl who can't live under the sun, are raised together when very young and become very attached to each other. One day, Eureka is taken away. Powerless at the time, Renton vows to rescue her. He enters the military and is soon is assigned to the Independent Youths Unit 303 of the First Mobile Forces thanks to his exceptional performance alongside his Nirvash, a bio-mechanical armor/control system. Unknown to Renton, lies a plot to extinguish the alien invasion that is currently happening involving not only him, but Eureka too.

国立爱丽丝研究机关学园本部不同于一般的学园，只招收具备特殊能力的学生，这种能力被称之为“爱丽丝”。因为好友今井萤（钉宫理惠 配音）转学从乡间来到了城里的爱丽丝学园，无论如何也不想和萤分开的佐仓蜜柑（植村加奈 配音）因此离家出走，跟随萤来到了学园。但没有超能力的她根本无法进入，被学院老师鸣海先生（石田彰 配音）救助后，意外地开发了蜜柑的超能力，于是，机缘巧合下，蜜柑也进入了爱丽丝学园，达成了她和萤在一起的愿望。
新学校的生活有喜有忧。蜜柑所具备的超能力被同学嗤笑为最无用能力，和其搭档的又是问题少年日向枣（朴璐美 配音），不能见相依为命的爷爷，在各种挫折困难面前，蜜柑依然乐观应对，逐渐赢得了大家的喜欢，也收获了和枣的爱情，但前路依旧有各种困难在等着他们……

Shouya Ishida starts bullying the new girl in class, Shouko Nishimiya, because she is deaf. But as the teasing continues, the rest of the class starts to turn on Shouya for his lack of compassion. When they leave elementary school, Shouko and Shouya do not speak to each other again... until an older, wiser Shouya, tormented by his past behaviour, decides he must see Shouko once more. He wants to atone for his sins, but is it already too late...?