In the present work, nanostructured perovskite oxides with improved reactivity, tunable morphology, and different forms (powder, thin films) were prepared using acrylic molecules such as acrylamide, acrylic acid, and methacrylic acid as novel chelating agents in a straightforward fashion. The approach, developed for LaCoO3, was also applied to oxides of the type LaMO3 (M = Fe, Ni), SrTiO3, and solid solutions thereof. The polymer-to-oxide evolution followed by XRD and IR showed merely a minimal amount of carbonate residuals even at temperatures as low as 600 °C. The different cross-linking degree of the polymeric compounds influenced the material crystallization leading to oxides with different grain sizes at the same calcination temperature. Among the prepared perovskites, acrylamide-derived LaCoO3 exhibited the highest oxygen surface reactivity as demonstrated by XPS and TPD measurements. As a result, the materials showed enhanced catalytic performance, leading to complete oxidation of CO at approximately 200 °C, which was almost 100 °C lower than for citric-acid-based samples. Finally, by exploiting the UV photopolymerization of the acrylic group, homogeneous, crystalline perovskite thin films of optical quality were successfully prepared through a straightforward spin-coating approach. The findings of this work demonstrate that this novel synthesis route is a better alternative to state-of-the-art citrate-based methods for the preparation of prospective catalysis, sensing, and energy conversion materials of high purity, activity, and tunable form.