Collaborative Filtering (CF) is a pivotal research area in recommender systems that capitalizes on collaborative similarities between users and items to provide personalized recommendations. With the remarkable achievements of node embedding-based Graph Neural Networks (GNNs), we explore the upper bounds of expressiveness inherent to embedding-based methodologies and tackle the challenges by reframing the CF task as a graph signal processing problem. To this end, we propose PolyCF, a flexible graph signal filter that leverages polynomial graph filters to process interaction signals. PolyCF exhibits the capability to capture spectral features across multiple eigenspaces through a series of Generalized Gram filters and is able to approximate the optimal polynomial response function for recovering missing interactions. A graph optimization objective and a pair-wise ranking objective are jointly used to optimize the parameters of the convolution kernel. Experiments on three widely adopted datasets demonstrate the superiority of PolyCF over current state-of-the-art CF methods. Moreover, comprehensive studies empirically validate each component's efficacy in the proposed PolyCF.