The fabrication of gradient ionogels for flexible strain sensors remains challenging because of the complex preparation procedures, and it is still difficult to prepare highly stretchable ionogels (strain > 10000%). In this study, a strategy is proposed to successfully fabricate gradient ionogels and apply them to flexible strain sensors by utilizing the self-floating character of the polysiloxane cross-linker. A gradient ionogel with ultrahigh stretchability (>14000%) is prepared via a one-step in situ photopolymerization process of the precursor with long-chain poly(dimethylsiloxane) bis(2-methyl acrylate) (PDMSMA). PDMSMA, which has a self-floating ability and excellent flexibility, induces a gradient composition distribution in the ionogel, thereby endowing the ionogel with superior stretchability and gradient changes in conductivity and adhesivity from the top to the bottom layer. Because of multiple molecular interactions, the bottom surface of the ionogel possesses good resilience and selfadhesion, whereas the top surface, which has a high PDMSMA content, shows a nonsticky performance. As a result, a singular gradient ionogel having both a sticky bottom surface and a nonsticky top surface is achieved. Furthermore, the flexible strain sensor that is created based on these gradient ionogels exhibits high sensitivity (its gauge factor reaching 5.08), a wide detection range (1− 1500%), fast response times, and good linearity. Notably, the detection signal remains repeatable over 1000 uninterrupted strain cycles. The fabricated strain sensor was further utilized to monitor joint movements and physiological signals. This work provides a facile strategy for fabricating gradient ionogels and shows their application potential in the field of flexible electronics.