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Cationic dendrimer assemblies with hierarchical structure, smart and biomimetic behaviors have been developed for drug\/gene delivery in vivo. Among different dendrimer assemblies, the dendrimer\u2010based nanogels were not intensively studied due to complicated synthesis and unknown properties. Here, for the first time, low\u2010generation dendrimer nanogels with high yield and purity, tunable size, uniform morphology, and good colloidal stability were synthesized using the emulsion\u2010free method, which cannot be obtained by the miniemulsion method. Importantly, the dendrimer nanogels integrate the advantages of low\u2010generation dendrimer and stimuli\u2010responsive polymer, thus achieving dual\u2010active groups,\n                    <jats:italic>o<\/jats:italic>\n                    \u2010hydroxyl amine units, temperature\u2010responsiveness, polyampholyte property, and self\u2010triggered aminolysis. With these unique properties, dendrimer nanogels can \u201ctemporarily\u201d acquire high charge density through the covalent crosslinking of low\u2010generation dendrimer for improved DNA compression, promoted cell internalization and lysosomal escape, and efficient DNA delivery, followed by self\u2010triggered aminolysis into small dendrimers to control DNA release, reduce cytotoxicity, and facilitate metabolism in vivo. Compared to high\u2010generation dendrimers, low\u2010generation dendrimer nanogels display higher gene transfection and therapeutic efficacies, and lower side effects simultaneously. This work provides a facile strategy for the preparation of low\u2010generation dendrimer nanogels that break up the contradiction between efficacy and cytotoxicity of cationic colloidal vectors in gene therapy. This innovative approach to construct low\u2010generation dendrimers into smart dendrimer nanogels will have broad applicability in clinical translation.\n                  <\/jats:p>","DOI":"10.1002\/anie.202505669","type":"journal-article","created":{"date-parts":[[2025,4,17]],"date-time":"2025-04-17T23:04:51Z","timestamp":1744931091000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":35,"title":["Functional Dendrimer Nanogels for DNA Delivery and Gene Therapy of Tumors"],"prefix":"10.1002","volume":"64","author":[{"given":"Xin","family":"Li","sequence":"first","affiliation":[{"name":"Institute of Technical and Macromolecular Chemistry RWTH Aachen University  52074 Aachen Germany"},{"name":"DWI\u2010Leibniz\u2010nstitute for Interactive Materials  52074 Aachen Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhijun","family":"Ouyang","sequence":"additional","affiliation":[{"name":"College of 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