This paper describes an Aerosol Robotic Network (AERONET)-based Surface Reflectance Validation Network (ASRVN) and its data set of spectral surface bidirectional reflectance and albedo based on Moderate Resolution Imaging Spectroradiometer (MODIS) TERRA and AQUA data. The ASRVN is an operational data collection and processing system. It receives 50 times 50 km2 subsets of MODIS level 1B (L1B) data from MODIS adaptive processing system and AERONET aerosol and water-vapor information. Then, it performs an atmospheric correction (AC) for about 100 AERONET sites based on accurate radiative-transfer theory with complex quality control of the input data. The ASRVN processing software consists of an L1B data gridding algorithm, a new cloud-mask (CM) algorithm based on a time-series analysis, and an AC algorithm using ancillary AERONET aerosol and water-vapor data. The AC is achieved by fitting the MODIS top-of-atmosphere measurements, accumulated for a 16-day interval, with theoretical reflectance parameterized in terms of the coefficients of the Li Sparse-Ross Thick (LSRT) model of the bidirectional reflectance factor (BRF). The ASRVN takes several steps to ensure high quality of results: 1) the filtering of opaque clouds by a CM algorithm; 2) the development of an aerosol filter to filter residual semitransparent and subpixel clouds, as well as cases with high inhomogeneity of aerosols in the processing area; 3) imposing the requirement of the consistency of the new solution with previously retrieved BRF and albedo; 4) rapid adjustment of the 16-day retrieval to the surface changes using the last day of measurements; and 5) development of a seasonal backup spectral BRF database to increase data coverage. The ASRVN provides a gapless or near-gapless coverage for the processing area. The gaps, caused by clouds, are filled most naturally with the latest solution for a given pixel. The ASRVN products include three parameters of the LSRT model (kL, kG, and kV), surface albedo, normalized BRF (computed for a standard viewing geometry, VZA = 0deg, SZA = 45deg), and instantaneous BRF (or one-angle BRF value derived from the last day of MODIS measurement for specific viewing geometry) for the MODIS 500-m bands 1-7. The results are produced daily at a resolution of 1 km in gridded format. We also provide a cloud mask, a quality flag, and a browse bitmap image. The ASRVN data set, including 6 years of MODIS TERRA and 1.5 years of MODIS AQUA data, is available now as a standard MODIS product (MODASRVN) which can be accessed through the Level 1 and Atmosphere Archive and Distribution System website ((http://ladsweb.nascom.nasa.gov/data/search.html).). It can be used for a wide range of applications including validation analysis and science research.