The implementation of aqueous electrode processing for lithium‐ion positive electrodes is key towards the realization of environmentally benign and cheap battery production. One of the water‐soluble binders that has attracted most attention is chitosan, the second‐most abundant natural biopolymer. Herein, the use of chitosan for high‐voltage, cobalt‐free LiNi$_{0.5}$Mn$_{1.5}$O$_{4}$ cathodes is reported for the first time. A detailed comparison of three different grades of chitosan with varying chain length and degrees of deacetylation (DD) is provided to explore the impact of these properties on the electrochemical performance. In fact, bio‐derived chitosan with a relatively lower DD outperforms synthetic chitosan‐especially after crosslinking with citric acid‐yielding about 10 % higher capacities. Higher molecular weight appears additionally advantageous for the cycling stability. Finally, guar gum is employed as slurry thickener, co‐crosslinking with chitosan. This allows for achieving 50 % higher mass loadings than for chitosan only and stable capacities above 130 and 120 mAh g$^{-1}$ at C/3 and 1 C, respectively.
