In　spintronics,　devices　exhibiting　large,　widely　tunable　magnetocurrent　(MC)　values　at　room　temperature　are　particularly　appealing　due　to　their　potential　in　advanced　sensing,　data　storage,　and　multifunctional　technologies.　Organic　semiconductors　(OSCs),　with　their　rich　and　unique　spin-dependent　and　(opto-)electronic　properties,　hold　significant　promise　for　realizing　such　devices.　However,　current　organic　devices　are　constrained　by　limited　design　strategies,　yielding　MC　values　typically　confined　to　tens　of　percent,　thereby　restricting　their　potential　for　multifunctional　applications.　Here,　this　study　introduces　an　electro-optical　compensation　strategy　to　modulate　MC　values,　which　synergistically　integrates　and　manages　the　interplays　among　carrier　transport,　spin-dependent　reactions,　and　photogenerated　carrier　dynamics　in　OSCs-based　devices.　This　approach　achieves　ultrahigh　room-temperature　MC　values　of　+13　200%　and　-10　600%　in　the　designed　devices,　with　continuous　and　precise　tunability　over　this　range-marking　a　breakthrough　in　organic　spintronic　devices.　Building　on　this　achievement,　by　integrating　multiple　controllable　parameters-light,　bias,　magnetic　field,　and　mechanical　flexibility-into　a　single　device,　a　flexible,　room-temperature,　multifunctional　device　is　activated,　functioning　as　the　high-sensitivity　magnetic　field　sensor,　composite　field　sensor,　magnetic　current　inverter,　and　magnetically-controlled　artificial　synaptic,　etc.　These　findings　open　an　avenue　for　designing　high-performance,　multifunctional　devices　with　broad　implications　for　future　spintronic-related　technologies.