Surface parameterization is a fundamental geometry processing task, laying the foundations for the visual presentation of 3D assets and numerous downstream shape analysis scenarios. Conventional parameterization approaches demand high-quality mesh triangulation and are restricted to certain simple topologies unless additional surface cutting and decomposition are provided. In practice, the optimal configurations (e.g., type of parameterization domains, distribution of cutting seams, number of mapping charts) may vary drastically with different surface structures and task characteristics, thus requiring more flexible and controllable processing pipelines. To this end, this paper introduces FlexPara, an unsupervised neural optimization framework to achieve both global and multi-chart surface parameterizations by establishing point-wise mappings between 3D surface points and adaptively-deformed 2D UV coordinates. We ingeniously design and combine a series of geometrically-interpretable sub-networks, with specific functionalities of cutting, deforming, unwrapping, and wrapping, to construct a bi-directional cycle mapping framework for global parameterization without the need for manually specified cutting seams. Furthermore, we construct a multi-chart parameterization framework with adaptively-learned chart assignment. Extensive experiments demonstrate the universality, superiority, and inspiring potential of our neural surface parameterization paradigm. The code will be publicly available at https://github.com/AidenZhao/FlexPara