This study introduces a novel single-diode rectenna, enhancing the rf-dc conversion efficiency using harmonic control of the antenna impedance. We employ source-pull simulations encompassing the fundamental frequency and the harmonics to achieve a highly efficient rectenna. The results of the source-pull simulations delineate the source-impedance ranges required for enhanced efficiency at each harmonic. Based on the source-pull simulation results, we designed two inverted-F antenna with input impedances within and without these identified source impedance ranges. Experimental results show that the proposed rectenna has a maximum rf-dc conversion efficiency of 75.9% at the fundamental frequency of 920 MHz, an input power of 10.8 dBm, and a load resistance of 1 kΩ, which is higher than that of the comparative rectenna without harmonic control of the antenna impedance. This study demonstrates that the proposed rectenna achieves high efficiency through the direct connection of the antenna and the single diode, along with harmonic control of the antenna impedance.