This paper presents the description of the wavelength modulation spectroscopy (WMS) experiment, the parameters of which were established by use of the Artificial Intelligence (AI) algorithm. As a result, a significant improvement in the signal power to noise power ratio (SNR) was achieved, ranging from 1.6 to 6.5 times, depending on the harmonic. Typically, optimizing the operation conditions of WMS-based gas sensors is based on long-term simulations, complex mathematical model analysis, and iterative experimental trials. An innovative approach based on a biological-inspired genetic algorithm (GA) and custom-made electronics for laser control is proposed. The experimental setup was equipped with a 31.23 m Heriott multipass cell, software lock-in, and algorithms to control the modulation process of the quantum cascade laser (QCL) operating in the long-wavelength-infrared (LWIR) spectral range. The research results show that the applied evolutionary approach can efficiently and precisely explore a wide range of WMS parameter combinations, enabling researchers to dramatically reduce the time needed to identify optimal settings. It took only 300 s to test approximately 1.39 × 10³² combinations of parameters for key system components. Moreover, because the system is able to check all possible component settings, it is possible to unquestionably determine the operating conditions of WMS-based gas sensors for which the limit of detection (LOD) is the most favorable.