The invention discloses a preparation method of a water treatment defluorination agent. The preparation method is characterized by comprising the following steps: step 1, preparing a sodium silicate solution, and adding a diluted hydrochloric acid solution for activation to obtain a solution A; step 2, weighing a first fixed amount of aluminum chloride hexahydrate solid, adding the aluminum chloride hexahydrate solid into the solution A, stirring for 10-30 minutes, continuously weighing a second fixed amount of ferric chloride hexahydrate solid, slowly adding the ferric chloride hexahydrate solid into the solution until the color of the solution becomes dark and turbid, continuously stirring, gradually clarifying the solution, and finally turning into a reddish brown transparent solution, so as to obtain a solution B; step 3, preparing a sodium carboxymethyl cellulose solution, namely a solution C; and step 4, placing the prepared solution B and the solution C in a constant-temperature water bath kettle according to the proportion, fully mixing and reacting in a high-speed stirring and heating state, and after the reaction is finished, obtaining the final defluorination agent solution. The fluorine removal rate of the deep defluorination agent can reach 95% or above, the fluorine removal rate is high, the fluorine removal effect is obvious, and deep fluorine removal of fluorine-containing wastewater can be achieved.