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We present the results of a comparison study in which a simple, automated, and unsupervised algorithm, which we call the arrange and average algorithm, was used to infer microphysical parameters (complex refractive index (CRI), effective radius, total number, surface area, and volume concentrations) of atmospheric aerosol particles. The algorithm normally uses backscatter coefficients (β) at 355, 532, and 1064 nm and extinction coefficients (α) at 355 and 532 nm as input information. We compared the performance of the algorithm for the existing “3β+α” and potential “3β+3α” configurations of a multiwavelength aerosol Raman lidar or highspectral-resolution lidar (HSRL). The “3β+3α” configuration uses an extra extinction coefficient at 1064 nm. Testing of the algorithm is based on synthetic optical data that are computed from prescribed CRIs and monomodal logarithmically normal particle size distributions that represent spherical, primarily fine mode aerosols. We investigated the degree to which the microphysical results retrieved by this algorithm benefits from the increased number of input extinction coefficients.