We propose a procedure to deconvolute the spectral power distribution (SPD) of phosphor-converted LEDs (pc-LEDs). The procedure involves a two-step process using multiple Gaussian functions. The first step is a preliminary process to deconvolute an SPD using a pair of Gaussian functions. Using the results from the first step, the second step determines (a) the number of Gaussian functions to be used in the analysis and (b) the initial values and regression domains of the coefficients of each Gaussian function for subsequent multiple-regression operations. Successful deconvolution is confirmed by comparing the values of lumen, correlated color temperature, and color rendering index with the experimental data of cool and warm pc-LEDs. The proposed approach is illustrated to evaluate the yellow-to-blue ratio and the phosphor power conversion efficiency.