“…As summarized in Tables [1][2][3][4], which are categorized by the types of materials, surface control can be multi-functional and act as inhibitors of phase transition, oxygen release and gas generation, protective barriers for electrolyte decomposition and TM dissolution, mechanical buffers, moisture and air shields, HF scavengers, and electronic/ionic conductivity facilitator, greatly enhancing the energy density, rate capability, cycle life, and safety [33]. Defining the chemical/physical/structural changes of the outer and inner surfaces as surface modification, three types can be categorized: (1) surface coating, the dominant strategies, including electrochemically inactive compounds coating (e.g., metal oxides, fluorides, and phosphates) [34][35][36][37][38], Li impurities-reactive coating (Co 3 O 4 ) [39] and Li-reactive coating (MoO 3 ) [40], Li ion conductive coating (LiTi 2 O 4 , Li 2 ZrO 3 and Li 4 -Mn 5 O 12 ) [41][42][43], conducting polymer coating (e.g., polypyrrole (PPy), polyaniline (PANI) and poly (3,4-ethylenedioxythiophene) (PEDOT)) [44][45][46], and other materials coatings, such as MXene (e.g. Ti 3 C 2 T x ) [47] and conductive graphene matrix [48]; (2) gradient structure design, including core-shell structures [49][50][51][52], hierarchical architectures (i.e., multi-shell) [53][54][55], and concentration gradient (CG) structures [56][57][58]; and (3) other surface treatments, such as rinsing with water to form an oxygendepleted surface layer [59,60], utilizing atomic surface reduction to alter the electronic structure of the surface …”