Federated learning (FL) has found many successes in wireless networks; however, the implementation of FL has been hindered by the energy limitation of mobile devices (MDs) and the availability of training data at MDs. How to integrate wireless power transfer and mobile crowdsensing towards sustainable FL solutions is a research topic entirely missing from the open literature. This work for the first time investigates a resource allocation problem in collaborative sensing-assisted sustainable FL (S2FL) networks with the goal of minimizing the total completion time. We investigate a practical harvesting-sensing-training-transmitting protocol in which energy-limited MDs first harvest energy from RF signals, use it to gain a reward for user participation, sense the training data from the environment, train the local models at MDs, and transmit the model updates to the server. The total completion time minimization problem of jointly optimizing power transfer, transmit power allocation, data sensing, bandwidth allocation, local model training, and data transmission is complicated due to the non-convex objective function, highly non-convex constraints, and strongly coupled variables. We propose a computationally-efficient path-following algorithm to obtain the optimal solution via the decomposition technique. In particular, inner convex approximations are developed for the resource allocation subproblem, and the subproblems are performed alternatively in an iterative fashion. Simulation results are provided to evaluate the effectiveness of the proposed S2FL algorithm in reducing the completion time up to 21.45% in comparison with other benchmark schemes. Further, we investigate an extension of our work from frequency division multiple access (FDMA) to non-orthogonal multiple access (NOMA) and show that NOMA can speed up the total completion time 8.36% on average of the considered FL system.