Black carbon (BC) aerosol emitted in incomplete combustion processes is known for causing warming in the climate system also poses serious health issues. Identification of the sources of BC is essential for the development of mitigation strategies to regulate their effects in changing climate. Among different observational and analytical techniques currently available, source apportionment methods based on optical measurements are relatively simple. For example, ‘Aethalometer model’ was developed based on Aethalometer observations. However, there are a few limitations with this model arising from assumption of wavelength and angstrom exponent pairs. We have developed an empirical method which also relies on Aethalometer observations named as ‘Two alpha method’ which assumes angstrom exponent from fossil fuel as 1 and estimates bio-mass fraction and angstrom exponent for bio-mass burning. This method has been applied to Aethalometer observations from five different locations (rural, semi-urban and urban) over Indian sub-continent to quantify sources of BC. Fossil fuel is found to be the major source of BC (∼70%) irrespective of the location. Collocated measurements of Carbon Monoxide (CO) over rural site correlated well with derived bio-mass fraction. Results from this study demonstrated the capabilities of empirical method and shall provide spatio-temporal variability in sources of BC if applied to more locations. An empirical method has been developed for source apportionment of black aerosol using Aethalometer observations. The results indicate fossil fuel as major source of BC. © 2019 Elsevier Ltd