Statistical models of crash frequency typically apply univariate regression models to estimate total crash frequency or crash counts by various categories. However, a possible correlation between the dependent variables or unobserved variables associated with the dependent variables is not considered when univariate models are used to estimate categorized crash counts—such as different severity levels or numbers of vehicles involved. This may lead to inefficient parameter estimates compared to multivariate models that directly consider these correlations. This paper compares the results obtained from univariate negative binomial regression models of property-damage only (PDO) and fatal plus injury (FI) crash frequencies to models using traditional bivariate and copula-based bivariate negative binomial regression models. A similar comparison was made using models for the expected crash frequency of single- (SV) and multi-vehicle (MV) crashes. The models were estimated using two-lane, two-way rural highway segment-level data from an engineering district in Pennsylvania. The results show that all bivariate negative binomial models (with or without copulas) outperformed the corresponding univariate negative binomial models for PDO and FI, as well as SV and MV, crashes. Second, the statistical association of various traffic and roadway/roadside features with PDO and FI, as well as SV and MV crashes, were not the same relative to their corresponding relationships in the univariate models. The bivariate negative binomial model with normal copula outperformed all other models based on the goodness-of-fit statistics. The results suggest that copula-based bivariate negative binomial regression models may be a valuable alternative for univariate models when simultaneously modeling two disaggregate levels of crash counts.