The　charm　embedded　in　nature　is　its　inherent　power　to　create　a　myriad　of　materials,　for　example,　a　spider　web　and　lotus　leaf,　with　ordinary　composition　but　exhibiting　fascinating　functional　property　owing　to　their　unique　structures.　Such　intricate　natural　designs　inspire　immense　research　in　synthesizing　materials　with　controlled　structure　and　morphology　toward　achieving　novel　or　enhanced　properties　for　target　applications.　Herein,　we　report　a　rotary　vacuum　evaporation　and　support-driven　nanoassembly　of　tiny　Pd　noble　metal　particles　on　nanosized　CeO2,　which　features　a　remarkable　unique　silk　＂mat-like＂　morphology　with　significant　anti-aggregation　of　Pd　nanoparticles　during　a　high　temperature　calcination　process,　whereas　the　obvious　aggregation　phenomenon　of　Pd　nanoparticles　occurs　when　using　commercial　CeO2　as　a　support.　This　nanocomposite　with　unique　structural　and　morphology　composition　is　able　to　act　as　a　highly　selective　and　active　visible　light　photocatalyst　toward　organic　redox　transformations　in　water,　including　aerobic　oxidation　of　alcohols　and　anaerobic　reduction　of　nitro-compounds　under　ambient　conditions,　representing　a　typical　tenet　of　photo　catalytic　green　chemistry.