An adsorbent (PEI‐GA) is prepared by crosslinking polyethyleneimine with glutaraldehyde. PEI‐GA shows outstanding adsorption performance towards Au(III) and Pd(II). PEI‐GA presents large adsorption capacity towards Au(III) in a wide application pH range from 1 to 9. The adsorption capacities of PEI‐GA for Au(III) and Pd(II) at 25°C reach 2575 and 497 mg/g, respectively. Au(III) and Pd(II) can be adsorbed completely within 10 min for 8.3 mg/L Au(III) and 20 min for 9.7 mg/L Pd(II). The adsorption equilibrium time required for 523.9 mg/L Au(III) and for 565.6 mg/L Pd(II) is 2 and 9 h, respectively. The Sips model is the most suitable to describe the adsorption isotherms which leads to more realistic adsorption capacities for both metals. PEI‐GA also exhibits high selectivity and repeatability towards Au(III) and Pd(II). The adsorption mechanism involves redox, chelation coordination, and electrostatic interactions for Au(III), and coordination and electrostatic interactions for Pd(II).