This article presents a gas sensing method based on long-tune natural logarithmic wavelength modulation spectroscopy (long-tune ln-WMS) and explores means to improve its accuracy. The long-tune spectrum can detect multiple gases with high precision. In ln-WMS, due to the natural logarithm algorithm, the harmonic magnitude which is related to gas concentration would not be affected by the light intensity fluctuations. However, the background signal of the harmonic will become strong and nonlinear in the long-tune spectrum. Three CO2 absorption lines and one H2O line near 2004 nm are applied to verify the proposed theory. The effects of light intensity, modulation depth, gas concentration, and phase shift on the harmonics are tested separately through both simulations and experiments. The results reveal that our proposed method can always keep the harmonics at their maximum which ensures high measurement precision. Moreover, the background signal only varies with the modulation depth, not the concentration and light intensity. Even the mechanical vibrations cannot disturb the harmonics, which enables the proposed method to be suitable for gas detection in harsh environments, especially for heavy dust and severe mechanical vibrations. The CO2 concentration detection results indicate that when the background is eliminated, the accuracy can be achieved with a relative error of below 0.5%, while the error would be greater than 5% with background presence. The proposed long-tune ln-WMS method is effective for trace gas detection (weak absorption) or over-modulation conditions and has potential applications in field inspection.