The fabrication of precise arrays of atoms is a key challenge at present. As a kind of biomacromolecule with strict base-pairing and programmable self-assembly ability, DNA is an idea material for directing atom positioning on predefined addresses. Here in this work, we propose the construction of iron atom arrays based on DNA origami templates and illustrate the potential applications in cryptography. First, ferrocene molecule is used as the carrier for iron atom since the cyclopentadienyl groups protect iron from being affected by the external environment. To characterize the iron atom arrays, streptavidins are labelled according to the ferrocene-modified DNA strand through biotin-streptavidin interactions. Based on atomic force microscopy scanning, ferrocene-modified single-stranded DNA sequences prove to be successfully immobilized on predefined positions on DNA origami templates with high yield. Importantly, the address information of iron atoms on origami is pre-embedded on the long scaffold, enabling the workload and cost to be lowered dramatically. In addition, the iron atom arrays can be used as the platform for constructing secure Braille-like patterns with encoded information. The origami assembly and pattern characterizations are defined as encryption process and readout process, respectively. The ciphertext can be finally decoded with the secure key. This method enables the theoretical key size of more than 700 bits to be realized. Encryption and decryption of plain text and a Chinese Tang poem prove the versatility and feasibility of this strategy.