Plasmonic-active nanomaterials are of high interest to scientists because of their expanding applications in the field for medicine and energy. Chemical and biological sensors based on plasmonic nanomaterials are well-established and commercially available, but the role of plasmonic nanomaterials on photothermal therapeutics, solar cells, super-resolution imaging, organic synthesis, etc. is still emerging. The effectiveness of the plasmonic materials on these technologies depends on their stability and sensitivity. Preparing plasmonics-active nanostructured thin films (PANTFs) on a solid substrate improves their physical stability. More importantly, the surface plasmons of thin film and that of nanostructures can couple in PANTFs enhancing the sensitivity. A PANTF can be used as a transducer for any of the three plasmonic-based sensing techniques, namely, the propagating surface plasmon, localized surface plasmon resonance, and surface-enhanced Raman spectroscopy-based sensing techniques. Additionally, continuous nanostructured metal films have an advantage for implementing electrical controls such as simultaneous sensing using both plasmonic and electrochemical techniques. Although research and development on PANTFs have been rapidly advancing, very few reviews on synthetic methods have been published. In this review, we provide some fundamental and practical aspects of plasmonics along with the recent advances in PANTFs synthesis, focusing on the advantages and shortcomings of the fabrication techniques. We also provide an overview of different types of PANTFs and their sensitivity for biosensing.