Thermoelectrics In article number 2103070, Sung-Yeon Jang, Ju-Won Jeon, and co-workers demonstrate selfhealable organic-inorganic ionic thermoelectric composites (OITCs) with unprecedentedly high ionic thermoelectric (TE) properties. It is discovered that the incorporation of inorganic nanoparticles promotes ion dissociation of ionic TE materials, which is crucial to improving ionic thermoelectric performance. Moreover, the OITCs can maintain their original ionic TE properties without noticeable degradation under repeated severe external strain and cutting/self-healing tests.