The albedo of seasonal snow cover plays an important role in the global climate system due to its influence on Earth's radiation budget and energy balance. Volunteer Community Collaborative Rain, Hail, and Snow-Albedo (CoCoRaHS-Albedo) observers collected 3249 individual daily albedo, snow depth and density measurements using standardized techniques at dozens of sites across New Hampshire, USA over four winter seasons. The data show that albedo increases rapidly with snow depth up to ~0.14 m. Multiple linear regression models using snowpack age, snow depth or density, and air temperature provide reasonable approximations of surface snow albedo during times of albedo decay. However, the linear models also reveal systematic biases that highlight an important non-linearity in snow albedo decay. Modeled albedo values are reasonably accurate within the range of 0.6–0.9, but exhibit a tendency to overestimate lower albedo values and underestimate higher albedo values. We hypothesize that rapid reduction in high albedo fresh snow results from a decrease in snow specific surface area, while during melt-events the presence of liquid water in the snowpack accelerates metamorphism and grain growth. We conclude that the CoCoRaHS-Albedo volunteer observer network provides useful snow albedo, depth and density measurements and serves as an effective model for future measurement campaigns.