Despite the high energy of LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode, it still suffers serious decay due to the continuous solvents decomposition and unstable cathode electrolyte interphase (CEI) layers, especially under high temperatures. The intense exothermic reaction between delithiated NCM811 and flammable organic solvents, on the other hand, pushes the batteries to their safety limit. Herein, we tackle these two issues via engineering the electrolytes, i.e., utilizing salts with higher HOMO levels and nonflammable solvents with lower HOMO levels, to reduce the massive decomposition of solvents on the cathode side and improve battery safety under elevated temperatures. Consequently, a thin and boron‐rich CEI was generated on the surface of NCM811, which effectively inhibited the side reactions and particle cracks, thus improving the cycling stability and safety. Deviated from the highly concentrated electrolytes which heavily relies on the usage of massive salts, our electrolyte recipe could introduce a robust inorganic‐rich CEI but use much less salt (i.e., dilute electrolyte), and thus, offer an encouraging alternative towards practical applications. As such, by adopting the proposed electrolyte, the NCM811 cathode exhibits a high‐capacity retention of 81.2% after 950 cycles at 25°C and 75% after 300 cycles at 55°C. This work provides a universal electrolyte design strategy for designing stable and safe high‐temperature electrolytes for the NCM811 cathode.This article is protected by copyright. All rights reserved