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A series of ambitious accessibility‐oriented policies have been launched in the world, which center around improving accessibility via the national multimodal transport systems including road, airline, and railway. The national multimodal transport accessibility assessment is one of the “basic” analyses for the design and implementation of these policies, whereas existing national‐scale accessibility studies either focus on single‐mode or two‐mode transport or ignore the schedule‐dependent nature of railway and airline. This article models the integrated road, railway, airline, and walking transport as a four‐layer network with the consideration of their interdependencies. An algorithm is then developed to accurately assess the travel time‐based accessibility on the four‐layer network with the consideration of the daily schedule of trains and flights. The proposed approach is applied to map accessibility to 363 cities in mainland China and analyze the optimal travel modes. In addition, this article investigates the travel time‐based vulnerability of the national multimodal transport system in mainland China under the extreme storm recently occurred in Zhengzhou (July 2021). The findings in this work provide insightful suggestions for transport planners to design the national multimodal transport systems and for stakeholders to schedule travels.