Abnormal bilirubin (BR) level is a sign of several fatal diseases, so it is of great significance and challenge to develop a facile and effective family routine strategy for BR sensing. Herein, novel water-stable Tb3+ @MOF-808 has been synthesized using a coordinated postsynthetic modification strategy and designed as a convenient and efficient fluorescence probe. The fabricated fluorescent probe exhibits a remarkable fluorescence quenching effect with the successive addition of BR, which displays fascinating features, such as fast response time, high sensitivity, and excellent selectivity. The quenching mechanism between the fluorescent probe and BR was also illustrated in detail. Importantly, the devised fluorescent probe successfully achieved the determination of BR in serum and urine, which has also been successfully used in the design of portable BR test paper. The developed monitoring platform for BR levels in vivo provides promising application potential for the prevention and early diagnosis of fatal diseases. Additionally, a molecular logic gate device that performs intelligent fluorescent sensing of BR was constructed. More interestingly, Tb3+@MOF-808 is used for development of latent fingerprints on different guest surfaces. The lines of the fluorescent fingerprints are clear and coherent, the details are obvious, and even sweat pores can be observed by naked eyes, which provides new means for tracking the criminal clue and handling cases efficiently.