We present high signal-to-noise, similar to5 Angstrom resolution (FWHM) spe
ctra of 66 z greater than or similar to 4 bright quasars obtained with the
4 m Cerro Tololo Inter-American Observatory and 4.2 m William Hershel teles
copes. The primary goal of these observations was to undertake a new survey
for intervening absorption systems detected in the spectra of background q
uasars. We look for both Lyman-limit systems (column densities N-HI greater
than or equal to 1.6 x 10(17) atoms cm(-2)) and damped Ly alpha systems (c
olumn densities N-IH greater than or equal to 2 x 10(20) atoms cm(-2)). Thi
s work resulted in the discovery of 49 Lyman-limit systems, 15 of which are
within 3000 km s(-1) of the quasar emission and thus might be associated w
ith the quasar itself, 26 new damped Ly alpha absorption candidates, 15 of
which have z >3.5, and numerous metal absorption systems. In addition, 10 o
f the quasars presented here exhibit intrinsic broad absorption lines.