• It is a comprehensive review on biomodified MOFs for various applications. • Functionalization of MOFs with amino acids and nucleic acids are summarized. • Biofunctionalization of MOFs exhibits structure- and function-specific applications. • It will inspire and promote the engineering/bioengimeering applications of MOFs. Metal-organic frameworks (MOFs) can be well-designed and constructed for various applications in gas storage and separation, heterogeneous catalysis, chemical sensing, and water remediation. To extend their applications in bio-related fields, the functionalization of MOFs with biomolecules such as DNA, proteins, peptides, enzymes, and others have been carried out, which improved the bioactivity and biocompatibility of MOF-biomolecule hybrid materials and enhanced the biomolecular recognition, targeting, and cell penetration of materials using the characteristics of bound biomolecules. In this review, we demonstrate the progress of MOF biofunctionalization with nucleic acid- (ssDNA, ds DNA, and aptamer) and amino acid-based biomolecules (single amino acid, peptide, and protein) for various structure- and function-specific applications. The methodologies on both covalent and noncovalent modifications of MOFs with nucleic acids and amino acids are introduced and summarized. More details on the conjugation of biomolecules onto MOFs for the function-specific applications in drug/gene delivery, tissue engineering, bioimaging, cancer therapy, biosensors, biocatalysis, separation, and nanomotors are demonstrated and discussed. We believe this work will be helpful for readers to understand the biofunctionalization of various MOFs with specific biomolecules and inspire the design and fabrication of novel MOF-based materials and devices for the applications in materials science and nanotechnology. [ABSTRACT FROM AUTHOR]