Magnetic composite fabricated from polyaniline and Fe3O4-hydrotalcite (Pan/MHT) was successfully applicated for removal of methyl orange (MO) from wastewater. The structure and properties of Pan/MHT were characterized by Fourier-transform infrared spectroscopy, scanning electron microscopy, X-ray diffraction, vibrating sample magnetometer, and Brunauer-Emmett-Teller adsorption isotherm. Adsorption kinetic results indicated that the adsorption process followed pseudosecond-order kinetic model (
R
2
=
0.999
), MO adsorption onto Pan/MHT was well described by Freundlich isotherm (
R
2
=
0.994
), and the MO adsorption capacity of 2 Pan/MHT obtained the highest with
Q
e
=
156.25
mg
/
g
. Batch adsorption experiments were carried out using magnetic composite with the effects of initial MO concentration, solution pH, and adsorbent dosage. The results revealed that the magnetic Pan/MHT exhibited efficient adsorption of MO in the aqueous solution as a result of the affinity for organic dyes, microporous structure, and suitable surface area for adsorption (15,460 m2/g). The superparamagnetic behavior of Pan/MHT (with
H
c
=
18.56
Oe
,
M
s
=
23.38
×
10
−
3
emu
/
g
, and
M
r
=
0.91
×
10
−
3
emu
/
g
) helps that it could be separated from the solution and performs as an economical and alternative adsorbent to removal and degrade azo dye from wastewater. Pan/MHT was also investigated to reuse after desorption of MO in 0.1 M HCl, and the results show that 2 Pan/MHT can be reused for 4 cycles with
Q
e
=
79.66
mg
/
g
.