Suburban railways have emerged as a predominant transport mode for suburbanization development in megacities. Enhancing transit-oriented development (TOD) in the catchment area of suburban railway stations is an essential strategy. To improve the catchment area identification, we proposed a method for delineating the catchment areas of suburban railway stations from the whole journey perspective and under a multi-mode access travel system. The grey distance delay (GDD) model was constructed to determine the catchment area. A case study was used to illustrate the applicability and advantages of our proposed method in metropolitan areas worldwide. The results indicated that the acceptable access distances vary greatly across access travel modes and are affected by the main travel in the suburban railway at the same time. The range of the catchment areas of bicycle and bus is larger than that of urban rail transit, and the strength of attraction of bicycle and bus shows a trend of increasing at first and then decreasing. Each access travel mode has its competitive advantage area, and these travel modes jointly serve the access trip within the suburban rail catchment area through a competition and cooperation relationship. These findings are able to enhance the identification of the catchment area and provide insights for suburban TOD and transport planning.