a b s t r a c tPlasmon resonances are widely used in biomolecular sensing and continue to be an active research field due to the rich variety of surface and measurement configurations, some of which exhibit down to single molecule level sensitivity. The resonance wavelength shift of the plasmonic structure upon binding of molecules, strongly depends, among other parameters, on how well the field of the resonant mode is confined to the binding site. Here it is shown that, by using properly designed metal-insulatormetal type resonators, improved wavelength response can be achieved with localized surface plasmon resonators (LSPRs) compared to that of the commonly used Kretschmann geometry. Using computational tools we investigate theoretically the refractive index response of several LSPR structures to a 2 nm thin film of binding molecules. LSPR resonators are shown to feature improved sensitivity over conventional Kretschmann geometry in the wavelength interrogation scheme for such a thin film. Moreover, some of the LSPR modes are quasi-omnidirectional and such angular independence (up to 30 • angle of incidence) allows higher numerical apertures to be used in colorimetric imaging. Results highlight the potential of LSPRs for biomolecular sensing with high sensitivity and high spatial resolution.