PA/PI‐ND exhibited charge and size switching capabilities. Charge responsiveness of a) MAL‐PEG‐PLL‐DMA, b) MAL‐PEG‐PLL‐TDA, and c) MAL‐PEG‐PLL‐CA incubated for different lengths of time and at different pH values (pH 7.4, 6.5, or 5.5). Size, zeta potential, and morphology of d) PA, e) PI, and f) PA/PI‐ND. g) Scheme of pH‐triggered disassembly of PA/PI‐ND. h) Zeta potential and size of PA/PI‐ND after incubation with PBS at different time‐periods and pH values. i) Zeta potential, size and j) morphology of PA/PI‐ND at different pH values after incubation for 1 h (Red circle represented disassembly of PA/PI‐ND). In vitro release behavior of k) abemaciclib and l) IMD‐0354 (*p < 0.05, **p < 0.01, ***p < 0.001, compared with PA/PI‐ND group under pH 7.4).