MgAC-Fe
3
O
4
/TiO
2
hybrid nanocomposites were synthesized in different ratios of MgAC-Fe
3
O
4
and TiO
2
precursor. X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray fluorescence spectrometry (XRF), electron spin resonance spectrometry (ESR), Brunauer-Emmett-Teller (BET), photoluminescence (PL), and UV photoelectron spectroscopy (UPS) were used to characterize the nanocomposites. The increase of MgAC-Fe
3
O
4
, in the hybrid nanocomposites’ core-shell structure, led to the decrease of anatase TiO
2
peaks, thus reducing the photo-Fenton and photocatalytic activities. According to the obtained data, MgAC-Fe
3
O
4
[0.05 g]/TiO
2
showed the best photo-Fenton and photocatalytic activities, having removed ~93% of MB (photo-Fenton reaction) and ~80% of phenol (photocatalytic reaction) after 20 and 80 mins, respectively. On the pilot scale (30 L), MgAC-Fe
3
O
4
[0.05 g]/TiO
2
was completely removed after 27 and 30 hours by the photo-Fenton and photocatalytic activities, respectively. The synergistic effect gained from the combined photo-Fenton and photocatalytic activities of Fe
3
O
4
and TiO
2
, respectively, was credited for the performances of the MgAC-Fe
3
O
4
/TiO
2
hybrid nanocomposites.