Periurban forests are key to offsetting anthropogenic carbon emissions, but they are under constant threat from urbanization. In particular, secondary Neotropical forest types in Andean periurban areas have a high potential to store carbon, but are currently poorly characterized. To address this lack of information, we developed a method to estimate periurban aboveground biomass (AGB)—a proxy for multiple ecosystem services—of secondary Andean forests near Bogotá, Colombia, based on very high resolution (VHR) GeoEye-1, Pleiades-1A imagery and field-measured plot data. Specifically, we tested a series of different pre-processing workflows to derive six vegetation indices that were regressed against in situ estimates of AGB. Overall, the coupling of linear models and the Ratio Vegetation Index produced the most satisfactory results. Atmospheric and topographic correction proved to be key in improving model fit, especially in high aerosol and rugged terrain such as the Andes. Methods and findings provide baseline AGB and carbon stock information for little studied periurban Andean secondary forests. The methodological approach can also be used for integrating limited forest monitoring plot AGB data with very high resolution imagery for cost-effective modelling of ecosystem service provision from forests, monitoring reforestation and forest cover change, and for carbon offset assessments.