CRUD depositions on fuel cladding are the main cause of power shift and localized corrosion in nuclear power plants. This paper is the first of a three-part study concerning the formation mechanism of CRUD depositions and its related heat transfer issues. In this paper, CRUD depositions are obtained under subcooled boiling conditions in 2 × 2 rod array channels via accelerated deposition method to explore corrosion product deposition and its feedback on heat transfer. Imbalance of deposition and erosion at initial stage causes fouling resistance to increase first and then decrease. CRUD growth is proposed as a relatively pure fouling process combining soluble precipitation and particulate aggregation. Through high-resolution characterizations, boiling chimney diameters span from 3 μm to a dozen microns. Principal components are nickel ferrite and nickel elemental with Fe/Ni ratio of 1.9:1. Static contact angle decreases to less than 30°. Effective CRUD thermal conductivity decreases with the increase of heat flux with 1.3866 W/(m × K) on average. The results of this study provide a precise method for understanding corrosion product deposition and its impact on heat transfer to further establish accurate CRUD-related models and predict CRUD-related safety issues.