The Monte Carlo method can be used to compute the gamma-ray backscattering albedo. This method was used by Raso to compute the angular differential albedo. Raso’s results have been used by Chilton and Huddelston to adjust their well-known albedo formula. Here, an efficient estimator is proposed to compute the double-differential angular and energetic albedo from gamma-ray histories simulated in matter by the three-dimensional Monte Carlo transport code TRIPOLI. A detailed physical albedo analysis could be done in this way. The double-differential angular and energetic gamma-ray albedo is calculated for iron material for initial gamma-ray energies of 8, 3, 1, and 0.5 MeV.