As a key factor in the design of a voltage-adjustable LLC resonant converter, frequency regulation range is very important to the optimization of magnetic components and efficiency improvement. This paper presents a novel optimal design method for LLC resonant converters, which can narrow the frequency variation range and ensure high efficiency under the premise of a required gain achievement. A simplified gain model was utilized to simplify the calculation and the expected efficiency was initially set as 96.5%. The restricted area of parameter optimization design can be obtained by taking the intersection of the gain requirement, the efficiency requirement, and three restrictions of ZVS (Zero Voltage Switch). The proposed method was verified by simulation and experiments of a 150 W prototype. The results show that the proposed method can achieve ZVS from full-load to no-load conditions and can reach 1.6 times the normalized voltage gain in the frequency variation range of 18 kHz with a peak efficiency of up to 96.3%. Moreover, the expected efficiency is adjustable, which means a converter with a higher efficiency can be designed. The proposed method can also be used for the design of large-power LLC resonant converters to obtain a wide output voltage range and higher efficiency.