We have designed and synthesized NaGdF 4 :Nd 3+ , Yb 3+ , Tm 3+ magnetic nanophosphors with combined dual-mode downconversion (DC) and upconversion (UC) photoluminescence upon 800 nm excitation. Hexagonal-phase NaGdF 4 :Nd 3+ , Yb 3+ , Tm 3+ nanocrystals (NCs) with an average size of 21 nm were synthesized using a solvothermal approach. Nd 3+ , Yb 3+ , Tm 3+ triple-doped NaGdF 4 NCs exhibit a broad range of photoluminescence peaks covering a near infrared first/second window (860-900, 1,000, and 1,060 nm), and visible emission including blue (475 nm), green (520 and 542 nm) and yellow (587 nm) after excitation at 800 nm. A mechanism involving circulation of energy over Gd 3+ sublattices as bridge ions and final trapping by the initial activator ions (Nd 3+ ) has been proposed. Penetration depth studies indicate that NIR emission is easily detected even at a large tissue thickness of 10 mm. These paramagnetic nanophosphors demonstrate a large magnetization value of 1.88 emu/g at 20 kOe and longitudinal relaxivity value of 1.2537 mM -1 ·S -1 as a T 1 -weighted magnetic resonance imaging contrast agent. These NaGdF 4 :Nd 3+ , Yb 3+ , Tm 3+ NCs are promising for applications in biological and magnetic resonance imaging.