Modern cosmology predicts that a galaxy overdensity (e.g., protocluster) will be associated with a large intergalactic medium gas reservoir, which can be traced by Lyα forest absorption. We have undertaken a systematic study of the relation between Coherently Strong intergalactic Lyα Absorption systems (CoSLAs), which have the highest optical depth (τ) in the τ distribution, and mass overdensities on the scales of ∼10-20 h −1 comoving Mpc. On such large scales, our cosmological simulations show a strong correlation between the effective optical depth (τ eff ) of the CoSLAs and the three-dimensional mass overdensity. In spectra with moderate signal-tonoise ratio, however, the profiles of CoSLAs can be confused with individual high column density absorbers. For z>2.6, where the corresponding Lyβ is redshifted to the optical, we have developed a selection technique to distinguish between these two alternatives. We have applied this technique to ∼6000 sight lines provided by Sloan Digital Sky Survey III quasar survey at z = 2.6-3.3 with a continuum-to-noise ratio greater than 8, and we present a sample of five CoSLA candidates with τ eff on 15 h −1 Mpc greater than 4.5× the mean optical depth. At lower redshifts of z<2.6, where the background quasar density is higher, the overdensity can be traced by intergalactic absorption groups using multiple sight lines with small angular separations. Our overdensity searches fully use the current and next generation of Lyα forest surveys, which cover a survey volume of >1 (h −1 Gpc) 3 . Systems traced by CoSLAs will yield a uniform sample of the most massive overdensities at z>2 to provide stringent constraints to models of structure formation.