Bike share system (BSS) has received increasing attention in research for its potential economic and environmental benefits. However, some research has pointed out the negative sustainability impacts of BSS from rebalancing activity, due to its greenhouse gas (GHG) emissions and additional vehicle travels. Additionally, bike and station manufacturing also bring considerable emissions to the system. Therefore, it is important to analyze the current rebalancing efficiency and sustainability of BSSs, and to assist the BSS operators in optimizing the BSS design. Existing studies lack tools to estimate the real-world rebalancing activities and vehicle usage for system sustainability evaluation and improvements. To address this gap, this research first proposed a framework to estimate rebalancing activities and applied a clustering-based method to estimate the rebalancing vehicle use. Applying the framework to the BSSs in Chicago, Boston, and Los Angeles, this study estimated the rebalancing operation and compared the rebalancing efficiencies among the three systems. The analysis results show that 1) only a small proportion of stations and bikes were involved in the daily rebalancing activities; 2) most rebalancing activities were operated during the daytime, while the overnight rebalancing was limited; 3) the system scale, trip demand, and station types are critical for the rebalancing efficiency; and 4) reducing the rebalancing activities at self-rebalance stations could help to improve the rebalancing efficiency and benefits system sustainability. Additionally, the sustainability performance (e.g., carbon emissions) of BSS is not only decided by the rebalance, but also the manufacturing of bikes and stations. It is important to consider all these factors when optimizing a BSS. The existing literature on system improvement for the BSSs lacks an integrated view, and a well-designed integrated model for current BSS improvement is needed. The second part of this thesis built a simulation-based optimization model and generated 2400 scenarios for evaluation. This model aims to minimize the expansion investment, rebalancing mileage, and maximize the system demand and service rate. A Weight Sum Model is applied to solve the multi-criteria decision analysis. The model results show that the best system improvement is to build a new station with a small capacity and initial bikes. The investment and location impacts are discussed to find the tradeoff among expansion strategies. A sensitivity analysis is conducted to evaluate how different weight combinations (refer to different preferences in decision making) impact the preferred station configuration (docks and bikes) and new station locations.