df["column"].value_counts(False).to_dict()

#Import dependencies
import numpy as np
import pandas as pd

#Create dataframe with random data
df = pd.DataFrame(np.random.randint(0,100,size=(100, 4)), columns=list('ABCD'))

#Create a 'result dataframe'
resultDf = pd.DataFrame(columns=list(df.keys()))

#Append value-count pairs to new dataframe
for column in df.keys():
    _dict_ = df[column].value_counts(False).to_dict()
    for index, key in enumerate(_dict_):
        resultDf.loc[index, column] = [key,_dict_.get(key)]