A multilayer network connection communication system includes a mobile device, a smart terminal device, a service server, a first layer network, and a second layer network. The mobile device sends at least one inquiry message through the first layer network to inquire the smart terminal device whether the smart terminal device supports at least one first application. Among the at least one first application, the smart terminal device supports at least one second application including a third application. The smart terminal device requests the mobile device through the first layer network to start up the at least one second application, where the third application is started up to respond to the at least one startup message. The smart terminal device receives a user data from the mobile device through the first layer network and transmits the user data to the service server through the second layer network.