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An increasing number of monitoring systems have been developed in smart cities to ensure that real-time operations of a city satisfy safety and performance requirements. However, many existing city requirements are written in English with missing, inaccurate, or ambiguous information. There is a high demand for assisting city policy makers in converting human-specified requirements to machine-understandable formal specifications for monitoring systems. To tackle this limitation, we build CitySpec, the first intelligent assistant system for requirement specification in smart cities. To create CitySpec, we first collect over 1,500 real-world city requirements across different domains from over 100 cities and extract city-specific knowledge to generate a dataset of city vocabulary with 3,061 words. We also build a translation model and enhance it through requirement synthesis and develop a novel online learning framework with validation under uncertainty. The evaluation results on real-world city requirements show that CitySpec increases the sentence-level accuracy of requirement specification from 59.02% to 86.64%, and has strong adaptability to a new city and a new domain (e.g., F1 score for requirements in Seattle increases from 77.6% to 93.75% with online learning).