MRI reporters for hyperpolarized 129Xe CEST need further improvement in order to sufficiently outcompete the intrinsic loss of hyperpolarization appearing under in vivo conditions. This study opens up a possibility by accelerating the CEST build-up for the well-known Xe host CrA-ma by two orders of magnitude. We designed a liposome decorated with a CrA-lipopeptide. To avoid inefficiency from back exchange, the lipopeptide fraction should be kept relatively low (e.g., 2 mol%). Complete saturation transfer could be easily achieved for maximum possible image contrast in 129Xe MRI scans. This study pinpoints a large flexibility for designing powerful HyperCEST agents.