Usually, there are several methods, e.g. experiment, interpolation experiment-based, analytic function, and Monte-Carlo simulation, to calculate the response functions in LaBr3(Ce) detectors. In logging applications, the experiment-based methods cannot be adopted because of their limitations. Analytic function has the advantage of fast calculating speed, but it is very difficult to take into account many effects that occur in practical applications. On the contrary, Monte-Carlo simulation can deal with physical and geometric configurations very tactfully. It has a distinct advantage for calculating the functions with complex configurations in borehole. A new application of LaBr3(Ce) detector is in natural gamma-rays borehole spectrometer for uranium well logging. Calculation of response functions must consider a series of physical and geometric factors under complex logging conditions, including earth formations and its relevant parameters, different energies, material and thickness of the casings, the fluid between the two tubes, and relative position of the LaBr3(Ce) crystal to steel ingot at the front of logging tube. The present work establishes Monte-Carlo simulation models for the above-mentioned situations, and then performs calculations for main gamma-rays from natural radio-elements series. The response functions can offer experimental directions for the design of borehole detection system, and provide technique basis and basic data for spectral analysis of natural gamma-rays, and for sonrceless calibration in uranium quantitative interpretation.