This paper focuses on how to synchronize network-wide timetables of first trains in an urban metro system, in which the train-connection-based route can be exactly determined for each first-train-attached origin-destination (OD) demand pair. With the help of even headway scheduling on each line, the problem is actually to adjust the departure times of first trains and connecting trains from their origin stations and the departure interval on each line. Subjected to train operation and connection constraints, a biobjective nonlinear integer programming model is formulated to minimize the total travel time of OD-dependent passenger demands and the deviation between the known and expected schedules. Then, the Nondominated Sorted Genetic Algorithm-II (NSGA-II) is adopted to solve the proposed model, and an improved technique is elaborated to reduce the alternative route choices. Finally, numerical experiments are conducted to demonstrate the effectiveness and availability of the proposed model and methods.