The development of a method for generating Sustainable Livelihood Security Index (SLSI) for agricultural sustainability and evaluating the existing status has been reported. Some measures have been suggested to promote sustainable agriculture of Orissa. This state has been selected since it faces wide inequality, improper management and over-exploitation of natural resources and explosion of population. These have created a threat to ecological balance and economic as well as social status of households in different districts of the state. The study of Ecological Security Index (ESI), Economic Efficiency Index (EEI) and Social Equity Index (SEI) has revealed that the agricultural systems of all districts display wide variations in their ecological and social equity aspects relative to their economic aspects. The districts with better SLSI ranks are often described as advanced districts and vice versa. Hence, SLSI has been found to reflect the picture of overall performance of a district in three dimensions of sustainability. On the basis of the overall performance of districts in terms of their SLSI, only eight districts in the state have an index value of more than 0.5, while thirteen districts have SLSI less than 0.4. Also, many districts of coastal Orissa have depicted better performance in agricultural sustainability in comparison to the districts of western Orissa as a whole. Some policy implications of SLSI approach have also been reported.