Cosmic-Ray Neutron Sensing (CRNS) is a novel technique for determining environmental water content by measuring albedo neutrons in the epithermal to fast energy range with moderated neutron detectors. We have investigated the response function of stationary and mobile neutron detectors typically used for environmental research in order to improve the model accuracy for neutron transport studies. Monte Carlo simulations have been performed in order to analyze the detection probability in terms of energy-dependent response and angular sensitivity for different variants of CRNS detectors and converter gases. Our results reveal the sensor’s response to neutron energies from 0.1 eV to 10⁶ eV and highest sensitivity to vertical fluxes. The detector efficiency shows good agreement with reference data from the structurally similar Bonner Spheres. The relative probability of neutrons contributing to the overall integrated signal is especially important in regions with non-uniform albedo fluxes, such as complex terrain or heterogeneous distribution of hydrogen pools