We release a database of cloze probability values, predictability ratings, and computational estimates for a sample of 205 English sentences (1726 words), aligned with previously released word-by-word reading time data (both self-paced reading and eye-movement records; Frank et al., Behavior Research Methods, 45(4), 1182–1190. 2013) and EEG responses (Frank et al., Brain and Language, 140, 1–11. 2015). Our analyses show that predictability ratings are the best predictors of the EEG signal (N400, P600, LAN) self-paced reading times, and eye movement patterns, when spillover effects are taken into account. The computational estimates are particularly effective at explaining variance in the eye-tracking data without spillover. Cloze probability estimates have decent overall psychometric accuracy and are the best predictors of early fixation patterns (first fixation duration). Our results indicate that the choice of the best measurement of word predictability in context critically depends on the processing index being considered.