df[df['Value']==df['Value'].max()]

This will return the entire row with max value

@DSM's answer is perfectly fine in almost any normal scenario. But if you're the type of programmer who wants to go a little deeper than the surface level, you might be interested to know that it is a little faster to call numpy functions on the underlying .to_numpy() (or .values for <0.24) array instead of directly calling the (cythonized) functions defined on the DataFrame/Series objects.

For example, you can use ndarray.max() along the first axis.

# Data borrowed from @DSM's post.
df = pd.DataFrame({"A": [1,2,3], "B": [-2, 8, 1]})
df
   A  B
0  1 -2
1  2  8
2  3  1

df['C'] = df[['A', 'B']].values.max(1)
# Or, assuming "A" and "B" are the only columns, 
# df['C'] = df.values.max(1) 
df

   A  B  C
0  1 -2  1
1  2  8  8
2  3  1  3 

If your data has NaNs, you will need numpy.nanmax:

df['C'] = np.nanmax(df.values, axis=1)
df

   A  B  C
0  1 -2  1
1  2  8  8
2  3  1  3 

You can also use numpy.maximum.reduce. numpy.maximum is a ufunc (Universal Function), and every ufunc has a reduce:

df['C'] = np.maximum.reduce(df['A', 'B']].values, axis=1)
# df['C'] = np.maximum.reduce(df[['A', 'B']], axis=1)
# df['C'] = np.maximum.reduce(df, axis=1)
df

   A  B  C
0  1 -2  1
1  2  8  8
2  3  1  3

np.maximum.reduce and np.max appear to be more or less the same (for most normal sized DataFrames)—and happen to be a shade faster than DataFrame.max. I imagine this difference roughly remains constant, and is due to internal overhead (indexing alignment, handling NaNs, etc).

The graph was generated using perfplot. Benchmarking code, for reference:

import pandas as pd
import perfplot

np.random.seed(0)
df_ = pd.DataFrame(np.random.randn(5, 1000))

perfplot.show(
    setup=lambda n: pd.concat([df_] * n, ignore_index=True),
    kernels=[
        lambda df: df.assign(new=df.max(axis=1)),
        lambda df: df.assign(new=df.values.max(1)),
        lambda df: df.assign(new=np.nanmax(df.values, axis=1)),
        lambda df: df.assign(new=np.maximum.reduce(df.values, axis=1)),
    ],
    labels=['df.max', 'np.max', 'np.maximum.reduce', 'np.nanmax'],
    n_range=[2**k for k in range(0, 15)],
    xlabel='N (* len(df))',
    logx=True,
    logy=True)