3D printing has attracted increasing interests in the field of metallic materials as it can effectively shorten the production cycle and create parts with complex shapes, which can hardly be produced by traditional methods. However, the gas atomization, as the mainstream method of preparing metal and alloy powders to meet the requirements of the processing of selective laser melting (SLM) at present, still has some limitations, such as hollow and/or satellite balls in the powder. This influences directly the density and performance of the printing parts. Moreover, the laser absorption in the smooth surface of powder particle is generally less than 10% in the laser processing, which hinders rapid heating of the powder. It has been found that the material can obtain multiple absorption of laser energy by increasing the surface roughness of powder particles, which can effectively improve the laser absorption rate and is beneficial to get the dense printing parts. Based on this, a novel method combining low temperature spray-drying with heat treatment was developed to prepare Ni powder with high purity, good sphericity, high flowability and narrow particle size distribution. The microstructure and laser absorptivity of the prepared Ni powder were compared with those of the commercial Ni powder prepared by gas atomization, and their influences on the microstructure and properties of the 3D printed bulk materials were investigated. It is found that the laser absorptivity of the Ni powder prepared by spray-drying is more than 2 times as high as that of the commercial Ni powder. This leads to a wider melting channel, smaller surface tension and liquid-bridging force between particles in the printing process. As a result, the spheroidization phenomenon occurred on the surface of the printed bulk material can be avoided by the use of the spray-dried powder, and the relative density is achieved as 99.2% at the as-printed state. In the microstructure of the printed bulk material, in addition to the cellular crystals, there are a number of fine columnar crystals, grown across the interlaminar boundaries, which is favorable for a high bonding strength between the interlayers.