Effective immobilization and delivery of genetic materials is at the forefront of biological and medical research directed toward tackling scientific challenges such as gene therapy, and cancer treatment. Here we present a biologically inspired hydrogen bonded zinc adeninate framework (ZAF) consisting of zinc adeninate macrocycles that self-assemble into a 3D framework via adenine-adenine interactions. ZAF can efficiently immobilize DNAzyme with full protection against enzyme degradation and physiological conditions until it is successfully delivered into the nucleus. Compared to zeolitic imidazolate frameworks (ZIFs), ZAFs are 2-folds more biocompatible with a significant loading efficiency of 96%. Overall, our design paves the way for expanding functional hydrogen-bonded-based systems as potential platforms for the loading and delivery of biologics.