Herein, a novel paper-based chemiluminescence (CL) assay is reported using a smartphone readout for on-site and reliable analytical applications. The CL system was based on the high-performance improving effect of cobalt-imidazole metal-organic framework (CoMOF) on luminol-hydrogen peroxide (H2O2) CL emission. The CoMOF was grown on paper and used as a support for the CL reaction, which led to an intense CL emission and good reproducibility. More importantly, the stability of luminol, as the CL reagent, was greatly improved in the presence of CoMOF. This high stability, along with the high-yield CL emission, makes the device highly suitable for commercialization. Furthermore, using a smartphone as the detector for the developed device made the process easier and more accessible for public usage. In this work, the new paper-based CL smartphone device was used for the detection of the total phenolic content of food samples. Phenolic compounds (PC) are hydroxyl radical scavengers that can effectively quench the CL emission of the luminol–H2O2–CoMOF system. After optimizing the reaction conditions, the system could detect PC at the μg mL−1 level. Detection limits of 0.12, 0.28, 0.46, 0.85, and 1.23 μg mL−1 were obtained for gallic acid, quercetin, catechin, kaempferol, and caffeic acid, respectively. This work is the first report on the practical application of smartphone CL assays for the estimation of PC. The proposed assay is an easy-to-use, low-cost, portable, and suitable assay for on-site screening purposes.