Tailoring optical properties of artificial metamaterials, whose optical properties go beyond the limitations of conventional and naturally occurring materials, is of importance in fundamental research and has led to many important applications such as security imaging, invisible cloak, negative refraction, ultrasensitive sensing, and transformable and switchable optics. Herein, by precisely controlling the size, symmetry, and topology of alphabetical metamaterials with U, S, Y, H, U-bar, and V shapes, we have obtained highly tunable optical response covering visible-to-infrared (vis-NIR) optical frequency. In addition, we show a detailed study on the physical origin of resonance modes, plasmonic coupling, the dispersion of resonance modes, and the possibility of negative refraction. We have found that all the electronic and magnetic modes follow the dispersion of surface plasmon polaritons; thus, essentially they are electronic- and magnetic-surface-plasmon-polaritons-like (ESPP-like and MSPP-like) modes resulted from diffraction coupling between localized surface plasmon and freely propagating light. On the basis of the fill factor and formula of magnetism permeability, we predict that the alphabetical metamaterials should show the negative refraction capability in visible optical frequency. Furthermore, we have demonstrated the specific ultrasensitive surface enhanced Raman spectroscopy (SERS) sensing of monolayer molecules and femtomolar food contaminants by tuning their resonance to match the laser wavelength, or by tuning the laser wavelength to match the plasmon resonance of metamaterials. Our tunable alphabetical metamaterials provide a generic platform to study the electromagnetic properties of metamaterials and explore the novel applications in optical frequency.