Objectives: Emphasizing the significance of optimal oral health for enhancing overall well-being, this study aimed to investigate oral health knowledge, self-assessed oral health behaviors, and oral hygiene practices within the Croatian general population. Materials and Methods: A cross-sectional observational study was conducted online, utilizing a questionnaire collecting sociodemographic characteristics and inquiring about respondents’ oral health knowledge, self-assessed oral health status, oral hygiene habits, and use of oral hygiene products. Collected data underwent both descriptive and regression analyses to unveil patterns and relationships within the dataset. Results: The respondents showed a high level of knowledge about oral health (median score 9, IQR 7.00–10.00, maximum possible score 10), with significant factors for higher knowledge being engaged in dental professions; above-average socioeconomic status; and the use of an electric brush, dental floss, and interdental brushes (p ˂ 0.05). Insufficient knowledge, on the other hand, was associated with bleeding gums and daily smoking (p ˂ 0.05). Although 69.4% of respondents considered their oral health to be very good, 32.5% reported tooth decay, and 38.2% reported tooth sensitivity. The majority (62.0%) cited regular check-ups as the reason for their last visit to the dentist, with 74.1% feeling no anxiety or discomfort during these visits. Daily toothbrush use was widespread (97.8%), but only 34.1% and 19.1% of respondents reported using floss and/or interdental brushes daily. A remarkable 69.0% of respondents indicated that low oral health literacy and low prioritization contribute to suboptimal oral health. Conclusions: While respondents demonstrated commendable oral health knowledge, the prevalence of reported issues suggests a potential gap between perception and actual oral health status. To address this, targeted educational interventions focusing on comprehensive oral hygiene practices and debunking misconceptions should be prioritized in Croatia.