Despite high charge capacity, iridium oxide (IrOx) coating is susceptible to delamination under prolonged stimulation, restricting its long‐term application. Here, a flower‐shaped platinum (Pt) nanocrystal with intensive high‐surface area is developed as an intermediate layer for accumulating IrOx (<3 wt% Ir) with enhanced adhesion, showing a multiplier effect. The impedance of IrOx/Pt flower coated microelectrode at 1 kHz is down to ≈2 kΩ (reduction of 94.23%). The corresponding cathodic charge storage capacity (CSCc) and charge injection capacity (CIC) are increased up to 202.75 ± 2.18 and 6.53 ± 0.16 mC cm–2, respectively. IrOx layer adheres tightly to Pt nanocrystals, demonstrating robust chronic stability under continuous electrostimulation for 1 × 108 cycles. Besides, the as‐prepared coatings show good biosafety, and exhibit promising electrocatalytic activity toward oxygen evolution reaction (OER) in 0.5 m sulfuric acid (H2SO4), requiring a low overpotential of ≈150 mV to reach 10 mA cm–2. IrOx helps in reducing the Tafel slope of Pt flower from 162.9 to 41.1 mV dec–1 drastically, also with excellent durability after chronoamperometry test. Excellent antibacterial properties toward Escherichia coli are also observed. This coating strategy provides a functionalized flexible electrode for neural interface, water oxidation, and anti‐microbial contamination, which will moreover extend to numerous applications.