The Sim Lab creates and studies living and lifelike soft materials through molecularly programmed self-assembly of synthetic polymers and engineered biological components. Self-assembly is how nature seamlessly integrates cellular functionalities with complex structures of materials. For example, plants, even a 300-foot-tall giant sequoia tree, are able to grow from a small seed because cellular division is coupled with material growth through self-assembly processes. The precision and specificity of chemical dialogues within these materials enable controlled growth, response, function, and adaptation characteristics, which are lacking in synthetic materials. In this presentation, I will introduce our studies in creating new types of living materials through molecularly programmed self-assembly of synthetic polymers with engineered cells and spores. I will discuss how this approach uniquely enables the seamless integration of living functionalities such as biocatalysis in materials and dynamic and controlled behaviors.