A new 4-acetalphenyl-substituted C
60
-pyrrolidine derivative, C
60
(C
12
H
17
NO
2
) (
1), has been prepared and its Langmuir films, with and without 22-tricosenoic acid [CH
2
![[double bond, length as m-dash]](https://www.rsc.org/images/entities/char_e001.gif)
CH–(CH
2
)
20
CO
2
H (TA)], at the air/water interface have been investigated. Pure
1 forms monolayers more easily than the parent molecule, C
60
, and can be transferred onto solid substrates to form Langmuir–Blodgett (LB) films. The mixed Langmuir films of
1 and TA were transferred onto hydrophilically pretreated quartz, glass substrates and silicon wafers. Reflectometric measurement of a 63-layer 1:2 mixed film on a silicon wafer using an He–Ne laser (
λ = 632.8 nm) provided a film thickness and refractive index of 171 nm and 1.73, respectively. Weak second harmonic generation (SHG) from LB monolayers of pure
1 and 1:2 and 1:4 mixed LB monolayer films of
1 and TA was observed. The second-order susceptibilities,
χ
pp
(2)
, were evaluated to be in the range (4–6)×10
−9
esu.