Considering interaction forces (gravity and buoyancy force, drag force, interaction potential force, and Brownian force) between nanoparticles and a base fluid, a two-phase Lattice Boltzmann model for natural convection of nanofluid is developed in this work. It is applied to investigate the natural convection in a square enclosure (the left wall is kept at a high constant temperature (TH), and the top wall is kept at a low constant temperature (TC)) filled with Al2O3/H2O nanofluid. This model is validated by comparing numerical results with published results, and a satisfactory agreement is shown between them. The effects of different nanoparticle fractions and Rayleigh numbers on natural convection heat transfer of nanofluid are investigated. It is found that the average Nusselt number of the enclosure increases with increasing nanoparticle volume fraction and increases more rapidly at a high Rayleigh number. Also, the effects of forces on nanoparticle volume fraction distribution in the square enclosure are studied in this paper. It is found that the driving force of the temperature difference has the biggest effect on nanoparticle volume fraction distribution. In addition, the effects of interaction forces on flow and heat transfer are investigated. It is found that Brownian force, interaction potential force, and gravity-buoyancy force have positive effects on the enhancement of natural convective heat transfer, while drag force has a negative effect.