Patient education materials (PEM)s were extracted from provincial cancer agencies to determine their organizational health literacy by evaluating the quality, actionability, and functional accessibility (e.g., readability and understandability) of their PEMs. PEMs from 10 provincial agencies were assessed for their grade reading level (GRL), using eight numerical and two graphical readability scales, and underwent a difficult word analysis. The agencies were assessed for PEM quality using two methods (JAMA benchmarks and DISCERN), while actionability and understandability were assessed using the Patient Education Materials Assessment Tool (PEMAT). Seven hundred and eighty-six PEMs were analyzed. The overall average GRL was 9.3 ± 2.1, which is above the recommended 7th GRL for health information. The difficult word analysis showed that 15.4% ± 5.1% of texts contained complex words, 35.8% ± 6.8% of texts contained long words, and 24.2% ± 6.6% of texts contained unfamiliar words. Additionally, there was high overlap between the most frequently identified difficult words in the PEMs and the most frequently misunderstood words by cancer patients identified in the literature. Regarding quality indicators, no agency displayed all four indicators according to the JAMA benchmarks and DISCERN scores ranged between 38 (poor) to 66 (excellent). PEMAT scores ranged between 68% to 88% for understandability and 57% to 88% for actionability. PEMs continue to be written at a level above the recommended GRL across all provinces, and there was overall high variability in the quality, understandability, and actionability of PEMs among provincial agencies. This represents an opportunity to optimize materials, thus ensuring understanding by a wider audience and improving health literacy among Canadian cancer patients.