The continuous increase in power density of electronic devices imposes stringent requirements on the design of lightweight, high-efficiency heat sinks. To overcome the limitations of conventional single-gradient or monomaterial heat sinks—namely, their suboptimal heat-transfer efficiency and poor structural adaptability—this study proposes a dual-gradient, triply periodic minimal surface (TPMS)-based multimaterial heat sink architecture fabricated from CuCrZr and AlSi₇Mg. Thermal performance was quantified experimentally using infrared thermography, while the underlying flow-field mechanisms were investigated numerically via computational fluid dynamics (CFD) simulations employing the standard k–ε turbulence model. With the TPMS material volume ratio fixed at 3:3 (CuCrZr:AlSi₇Mg), the Z-axis gradient configuration P-Z4-5 delivered the best overall thermal performance, achieving a heat-transfer coefficient (HTC) of 1557.63 W·m⁻²·K⁻¹ and a thermal resistance as low as 1.83 K·W⁻¹ at an inlet velocity of 5 m·s⁻¹. In contrast, the Y-axis gradient configuration P-Y3-6 yielded the most uniform temperature distribution, exhibiting a maximum surface temperature difference of only 21.5 °C under the same inlet condition. Velocity and turbulence distribution analyses reveal that the dual-gradient design enhances both the narrow-tube effect and flow-induced disturbances; furthermore, increasing the inlet velocity from 5 m·s⁻¹ to 21.65 m·s⁻¹ significantly intensifies vorticity-driven fluid mixing. Among all configurations evaluated, P-Z4-5 exhibited the highest j/f factor (i.e., the ratio of Colburn j-factor to Fanning friction factor), followed by P-Z3.5-5.5 and P-Z3-6. These findings establish a promising new pathway for the development of high-performance, lightweight heat sinks tailored for next-generation high-power electronics.