Following a novel approach, the vertical distributions of columnar aerosol optical depth (AOD), precipitable water content (PWC) and ozone (TCO) have been determined using compact, multi-filter, solar radiometers during winter period of 2002–2003. These profiles were obtained by making measurements at different altitudes while ascending to/descending from a rural site, elevated up to an altitude of about 1450 m above mean sea level (AMSL). Besides the wavelength dependency, the profiles depict significant layer structures which are explained on the basis of concurrent atmospheric stability parameters. The aerosol size distributions which were obtained from the inversion of spectral dependence of AOD at different altitudes show a mixture of power-law, mono- and bi-model distributions indicating the influence of aerosols originating from both anthropogenic and natural sources. The present results, representing a rural high-altitude station, are compared with those reported over a few selected similar high-altitude stations in North India, and also observed at a nearby urban station (Pune) in Central India to infer modulation of terrain-induced meteorological parameters on aerosol source strength. The importance of the experimental approach and profiles of AOD and pre-cursor gases over areas with scarce alternative measurements, networks with sporadic presence of ground sites and limited number of satellite retrievals is highlighted.